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Structural evolution of ZIF-67-derived catalysts for furfural hydrogenation

Jun Gyeong Lee, Sinmyung Yoon, Euiseob Yang, Jae Hwa Lee, Kyung Song, Hoi Ri Moon, Kwangjin An
Journal of catalysis 2020 v.392 pp. 302-312
active sites, carbon, catalysts, catalytic activity, coordination polymers, correlation, evolution, exhibitions, furfural, furfuryl alcohol, hydrogenation, nanoparticles, oxidation, particles, surface area, temperature, yields
Zeolitic imidazolate framework-67 (ZIF-67) can be converted to metallic Co nanoparticles supported on N-doped carbon (Co/NC) through reduction. However, its unique properties, including extremely high surface area, isoreticular pore structure, and regular metal–organic network, disappear after high-temperature (>500 °C) reduction. Aggregated CoOₓ particles reduce the number of surface-active sites, resulting in poor catalytic activity. If the original ZIF-67 structure is maintained after the high-temperature reduction, promoting the uniform distribution of active sites in the porous carbon, the catalytic performance can be further improved. Herein, the correlation between the catalytic furfural hydrogenation performance, Co/NC morphology, and oxidation state of Co was investigated as a function of the H₂ reduction temperature and time. The reduction of ZIF-67 at 400 °C for 6 h yields a highly dispersed Co/NC catalyst, while preserving the overall morphology. The resulting Co/NC-400-6 catalyst exhibits the highest activity, promoting high selectivity toward 2-methylfuran. The product selectivity can be further altered by incorporating Cu into ZIF-67 to produce furfuryl alcohol. With proper H₂ treatment to minimize the damage to the intrinsic surface area and pore structure, metal–organic frameworks can be utilized as high-performance heterogeneous catalysts by maximizing the distribution of active sites.